Manipulating
catalytic
active
sites
and
reaction
kinetics
in
alkaline
media
is
crucial
for
rationally
designing
mighty
water-splitting
electrocatalysts
with
high
efficiency.
Herein,
the
coupling
between
oxygen
vacancies
interface
engineering
highlighted
to
fabricate
a
novel
amorphous/crystalline
CrOx
-Ni3
N
heterostructure
grown
on
Ni
foam
accelerating
hydrogen
evolution
(HER)
(OER).
Density
functional
theory
(DFT)
calculations
reveal
that
electron
transfer
from
amorphous
Ni3
at
interfaces,
optimized
Gibbs
free
energies
of
H2
O
dissociation
(ΔGH-OH
)
H
adsorption
(ΔGH
are
conducive
superior
stable
HER
activity.
Experimental
data
confirm
numerous
interfaces
catalysts
favorable
abundant
accessible
enhanced
intrinsic
activity,
resulting
excellent
performances
OER.
Additionally,
situ
reconstruction
into
highly
N/Ni(OH)2
responsible
OER
performance
long-term
stability
test.
Eventually,
an
electrolyzer
using
as
both
cathode
anode
has
low
cell
voltage
1.53
V
10
mA
cm-2
,
together
extraordinary
durability
500
h,
revealing
its
potential
industrial
applications.
Energy & Environmental Science,
Год журнала:
2021,
Номер
14(4), С. 1897 - 1927
Опубликована: Янв. 1, 2021
The
review
summarizes
transition
metal-based
bimetallic
MOFs
and
their
derived
materials
as
electrocatalytic
for
the
OER.
mechanisms
of
OER
probed
by
DFT
calculation
andin
situcharacterization
techniques
are
also
discussed.
Energy & Environmental Science,
Год журнала:
2021,
Номер
14(6), С. 3393 - 3419
Опубликована: Янв. 1, 2021
Understanding
the
durability-limiting
factors
of
anion
exchange
membrane
water
electrolyzers
operating
under
pure
water-,
KOH-
and
K2CO3-fed
conditions.
Energy & Environmental Science,
Год журнала:
2023,
Номер
16(4), С. 1384 - 1430
Опубликована: Янв. 1, 2023
This
review
presents
the
state-of-the-art
MEAs,
including
key
components
and
preparation
technologies.
Especially,
overall
design
strategies
of
MEAs
are
discussed
to
promote
high-performance
alkaline
water
electrolysis.
Chemical Reviews,
Год журнала:
2023,
Номер
123(9), С. 5347 - 5420
Опубликована: Апрель 12, 2023
Enzymatic
catalysis
has
fueled
considerable
interest
from
chemists
due
to
its
high
efficiency
and
selectivity.
However,
the
structural
complexity
vulnerability
hamper
application
potentials
of
enzymes.
Driven
by
practical
demand
for
chemical
conversion,
there
is
a
long-sought
quest
bioinspired
catalysts
reproducing
even
surpassing
functions
natural
As
nanoporous
materials
with
surface
areas
crystallinity,
metal-organic
frameworks
(MOFs)
represent
an
exquisite
case
how
enzymes
their
active
sites
are
integrated
into
porous
solids,
affording
heterogeneous
superior
stability
customizable
structures.
In
this
review,
we
comprehensively
summarize
advances
MOFs
catalysis,
discuss
design
principle
various
MOF-based
catalysts,
such
as
MOF-enzyme
composites
embedded
sites,
explore
utility
these
in
different
reactions.
The
advantages
enzyme
mimetics
also
highlighted,
including
confinement,
templating
effects,
functionality,
comparison
homogeneous
supramolecular
catalysts.
A
perspective
provided
potential
solutions
addressing
current
challenges
MOF
catalysis.
ACS Catalysis,
Год журнала:
2023,
Номер
13(4), С. 2313 - 2325
Опубликована: Янв. 30, 2023
Single-atom
introduced
carbon
nanomaterials
show
favorable
oxygen-reduction
reaction
(ORR)
and
oxygen-evolution
(OER)
performance
for
renewable
energy
applications.
Nevertheless,
the
electronic-structure
regulation
by
decorating
heterogeneous
single-metal-atoms
engineering
of
a
single-atom
active-sites'
microenvironment
need
to
be
optimized
simultaneously,
which
is
challenging.
Herein,
we
develop
an
atomic-interfacial-regulation
approach
fabricate
dual
single
Fe/Co
atoms
synchronized
with
both
nitrogen/sulfur
on
defective/graphitic/porous
nanosheets
(Fe,Co/DSA-NSC).
The
unsymmetrically
organized
N
S
coordinated
bridged
atomic-sites
[Fe-(N2S)/Co-(N2S)
moiety]
are
established
prompt
charge-transfer,
lowering
barrier
oxygenated
reaction-intermediates
leading
boost
reaction-kinetics.
As
estimated,
Fe,Co/DSA-NSC
exhibits
improved
ORR/OER
activity
higher
half-wave
potential
lower
overpotential
(E1/2
=
879
mV
η10
210
mV,
respectively)
also
good
cycling
stability
toward
zinc-air
batteries.
This
discovery
hence
provides
widespread
scheme
synergistic-principles
dual-single-atom
catalysts
controlled
Journal of Materials Chemistry A,
Год журнала:
2021,
Номер
9(24), С. 14043 - 14051
Опубликована: Янв. 1, 2021
Developing
practical
water-splitting
devices
that
convert
earth-abundant
solar
energy
and
water
into
renewable
fuel
holds
promise
for
a
sustainable
future;
however,
its
successful
commercialization
applications
is
limited
by
the
sluggish
kinetics
of
oxygen
evolution
reaction
(OER).
Herein,
we
developed
high-efficiency
low-cost
three-dimensional
(3D)
OER
electrode
via
electrochemical
integration
amorphous
NiFeOOH
on
surface
activated
carbon
fiber
paper
(CFP).
The
as-synthesized
3D-a-NiFeOOH/N-CFP
exhibits
an
ultra-low
overpotential
η(O2)
170
mV
to
afford
10
mA
cm−2
current
density,
together
with
Tafel
slope
39
per
decade,
excellent
stability
under
conditions.
Apart
from
synergistic
effect,
activity
a-NiFeOOH/N-CFP
attributed
unique
3D
structure
enriched
active
sites
improved
electrical
conductivity
facilitates
fast
mass
transport
properties.
As
result,
catalyst
achieves
high
turnover
frequency
(TOF)
0.99
s−1
(jm)
2527
A
g−1
at
270
mV,
which
outperforms
so
far
reported
state-of-the-art
catalysts
commercial
IrO2.
Besides,
alkaline
anion
exchange
membrane
electrolyzer
fabricated
anode
delivers
1
1.88
V
long-term
durability
240
h.
These
findings
highlight
design
significant
advancements
towards
utilization
applications.